AutoDFT: A Closed-Loop Multi-Agent Framework for Autonomous DFT Calculations

ArXi:2605.26179v1 Announce Type: cross Density functional theory (DFT) serves as the basis for computational discovery in materials science and chemistry, yet each calculation demands extensive human effort: adjusting algorithms when convergence stalls, revising plans when unexpected physics emerges, and inserting steps as intermediate results reshape the problem. Existing LLM-based agents automate only the initial planning stage, producing a full execution plan upfront and leaving all subsequent adaptation to hand-crafted rules.